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The main uncertainties regarding the estimation of changes in the Earth's energy budget are related to the role of atmospheric aerosols. These changes are caused by aerosol–radiation (ARIs) and aerosol–cloud interactions (ACIs), which heavily depend on aerosol properties. Since the 1980s, many international modeling initiatives have studied atmospheric aerosols and their climate effects. Phase 3 of the Air Quality Modelling Evaluation International Initiative (AQMEII) focuses on evaluating and intercomparing regional and linked global/regional modeling systems by collaborating with the Task Force on the Hemispheric Transport of Air Pollution Phase 2 (HTAP2) initiative. Within this framework, the main aim of this work is the assessment of the representation of aerosol optical depth (AOD) and the Ångström exponent (AE) in AQMEII Phase 3 simulations over Europe. The evaluation was made using remote-sensing data from the Moderate Resolution Imaging Spectroradiometer (MODIS) sensors aboard the Terra and Aqua platforms, and the instruments belonging to the ground-based Aerosol Robotic Network (AERONET) and the Maritime Aerosol Network (MAN). Overall, the skills of AQMEII simulations when representing AOD (mean absolute errors from 0.05 to 0.30) produced lower errors than for the AE (mean absolute errors from 0.30 to 1). Regardless of the models or the emissions used, models were skillful at representing the low and mean AOD values observed (below 0.5). However, high values (around 1.0) were overpredicted for biomass burning episodes, due to an underestimation in the common fires' emissions, and were overestimated for coarse particles – principally desert dust – related to the boundary conditions. Despite this behavior, the spatial and temporal variability of AOD was better represented by all the models than AE variability, which was strongly underestimated in all the simulations. Noticeably, the impact of the model selection when representing aerosol optical properties is higher than the use of different emission inventories. On the other hand, the influence of ARIs and ACIs has a little visible impact compared to the impact of the model used. [ABSTRACT FROM AUTHOR]

Analysis of the stable carbon isotope 13C in organic carbon (OC) can give insight into sources and atmospheric processing of carbonaceous aerosols, provided the 13C source signatures are known. However, only few data on 13C signatures of OC emitted by common sources of carbonaceous aerosol are available in Europe. We present and evaluate an improved version of a measurement method to obtain δ 13C signatures on organic aerosols desorbed from filter samples at three different desorption temperatures (200 °C, 350 °C and 650 °C) and apply it in a source study. With our calibration approach, the reproducibility of a L-Valine reference material desorbed at a single temperature step of 650 °C shows a standard deviation of 0.19‰ over a period of more than one year. The average δ 13C value for this reference material over 248 measurements is −24.10‰, which shows only a slight bias to the nominal value of −24.03‰. Repeated analysis of ambient filter samples desorbed at three temperature steps show typical standard deviations of about 0.3‰ for all temperature steps (200 °C, 350 °C and 650 °C). Isotopic fractionation due to partial thermal desorption during the individual temperature steps was tested on single compound reference materials. It showed significant isotopic fractionation only at temperature steps, in which a very minor fraction of the compound was desorbed. Possible isotope effects caused by charring of organic material were investigated and found to be not significant. The thermal desorption method was applied to various source filter samples from the region of Naples, Italy. We analyzed two different biomass burning sources, exhaust from a city bus and traffic emissions collected in a tunnel and compared these to ambient filter samples from the same region. δ 13C signatures of the total OC show values in a narrow range of about −28‰ to −26‰ for all sources, which does not allow a source apportionment only based on 13C. Nevertheless, the results add information to a source inventory of δ 13C, where information of 13C in organic aerosol from specific emission sources are rare. City bus emissions show little variation of δ 13C over the temperature steps, whereas biomass burning aerosol is enriched in 13C for OC desorbed at 650 °C. For PM10 samples in the urban tunnel an enrichment in δ 13C at the 650 °C temperature steps was observed, which is likely caused by the contribution of carbonate carbon to the carbonaceous material desorbed at this temperature step. • Stable method to analyze δ13C of organic aerosol at several desorption temperatures. • Charring/isotopic fractionation during thermal desorption do not influence δ13C(OC). • δ13C value of ambient filters is in the range of emission sources in Naples, Italy. • carbonate carbon causes enrichment in δ13C at 650 °C for ambient and tunnel filter. [ABSTRACT FROM AUTHOR]

• Aerosol fluxes over a forest showed a strong seasonal and size-dependent variation. • Leaf-presence drove fine particles deposition and ultrafine particles emission. • Deposition velocity of ultrafine and fine particles correlated with leaf area index. • Plant stomatal activity seemed to influence the emission of ultrafine particles. • Deposition of accumulation mode aerosols was related to impaction processes. Eddy covariance measurements of aerosol fluxes were performed above an oak-hornbeam forest in the Po Plain (Northern Italy), from February to May and from September to December 2019. Measurements aimed at assessing the influence of forest phenology and leaf presence/absence on the seasonal evolution of size-segregated aerosol fluxes. The size-resolved aerosol concentration in the range 0.006-10 μm was sampled with a 14-stage impactor (ELPI+, Dekati, FI), and the filters exposed in May were subjected to chemical analysis. Over the whole sampling period, the forest removed from the atmosphere an average of 3.12 mg of aerosol m−2 d−1. The direction and the intensity of the aerosol fluxes were not constant through the year, as a strong seasonal and size-dependent variability emerged. In particular, leaf-presence drove a net deposition of the accumulation mode aerosol (100 nm< particle diameter D p <1000 nm) and an emission of the Aitken (10 nm< Dp<100 nm) and coarse mode (Dp>1000 nm) aerosols. On the contrary, in absence of leaves all the sub-micrometer aerosol size-classes showed net daily upward fluxes, while coarse mode aerosol fluxes were prevalently downward. Monthly averages of deposition velocities of Aitken and accumulation mode aerosols correlated with the Leaf Area Index (LAI) seasonal trend, thus indicating an important role of the amount of the leaf surface area on the deposition and emission of these size-classes. Furthermore, an influence of the stomatic activity was suggested for the Aitken mode aerosol, since its deposition velocity followed the same diel course of the stomatal conductance to water. The analysis of the influence of meteorological parameters on aerosol deposition velocities highlighted that dynamic and convective turbulence (described by friction velocity, u* and Deardorff velocity, w*) enhanced the vertical aerosol exchanges, both upward and downward, while the approaching of condensing conditions reduced the flux intensities. [ABSTRACT FROM AUTHOR]

The paper presents eddy covariance measurements of aerosol fluxes performed above an Alpine pasture in the Camonica Valley (Italian Alps) during summer 2019 and winter 2020. Vertical fluxes and deposition velocities (v d s) were computed for nine aerosol size classes, with geometric mean diameters (GMDs) ranging from 10 nm to 0.76 μm, employing a fast-response electrical low-pressure impactor (ELPI+, Dekati, FI). At the end of each campaign, the concentration of water-soluble ions was estimated from the ion chromatography chemical speciation performed on the multi-impactor filters. K+ concentrations tripled in winter, evidencing the impact of biomass burning emissions, while nitrate, nitrite, ammonium, and sulphate were ascribed to secondary inorganic aerosol (SIA) formation. During summer, classes characterized by downward net daily fluxes presented a high percentage of SIA (> 70%) deposited on the respective filters. Phenomena of growth or coagulation of particles were also detected from the steady increase in concentrations during the day in classes with GMD ≥ 20 nm. Turbulence favoured intense aerosol exchange during the day. During summer nights, low friction velocities (u ∗) led to weaker fluxes, while a strong, stable stratification in winter determined aerosol trapping at ground level and non-negligible, mostly negative, fluxes during nighttime. The trends of v d s versus aerosol GMDs showed prevailing deposition phenomena under stable atmospheric conditions, with relative humidity higher than or equal to 90%, friction velocity lower than 0.15 m s−1, or wind speed lower than 2 m s−1. Cluster analysis identified groups of days with or without nucleation events and highlighted a rainout effect in summer during a period characterized by intense precipitation. • Aerosol fluxes are evaluated in summer and winter on an Alpine valley floor. • Alpine pastures contribute to the formation of secondary inorganic aerosol. • Nucleation and growth processes lead to deposition fluxes. • Seasonal emission sources lead to upward fluxes. • Aerosol is mostly deposited under stable conditions. [ABSTRACT FROM AUTHOR]